This dissertation, through a systematic investigation of the behavior of the gas-phase dynamics ofnanoparticles generated by laser ablation of solid target materials in background gasesand a study of the physical processes involved in gas-phase nanoparticle processing, explores the combination of laser and aerosol processes as a novel approach to make thinfilm materials with a level of microscopic organization similar to that found in nature.The integrated laser-aerosol method is very flexible and can be used in thesynthesis of a variety of materials. In this study it is applied to the deposition ofnanocomposite thin films comprising tetrahedral amorphous carbon (ta-C) withembedded metal nanoparticles. The controlled incorporation of metal nanoparticlesenables the modulation of the electrical conductivity of ta-C over four orders ofmagnitude without significantly or adversely affecting its mechanical properties.